scholarly journals How do Cl concentrations matter for simulating CH<sub>4</sub>, δ<sup>13</sup>C(CH<sub>4</sub>) and estimating CH<sub>4</sub> budget through atmospheric inversions?

2021 ◽  
Author(s):  
Joël Thanwerdas ◽  
Marielle Saunois ◽  
Isabelle Pison ◽  
Didier Hauglustaine ◽  
Antoine Berchet ◽  
...  
Keyword(s):  
Seasonal Cycle ◽  
Recent Literature ◽  
Isotopic Signature ◽  
Atmospheric Methane ◽  
Top Down ◽  
Total Oxidation ◽  
Sources And Sinks ◽  
Cycle Amplitude ◽  
Additional Constraints ◽  
Atmospheric Inversions

Abstract. Atmospheric methane (CH4) concentrations have been rising since 2007, resulting from an imbalance between CH4 sources and sinks. The CH4 budget is generally estimated through top-down approaches using CH4 observations as constraints. The atmospheric isotopic CH4 signal, δ13C(CH4), can also provide additional constraints and helps to discriminate between emission categories. The oxidation by chlorine (Cl) likely contributes less than 5 % to the total oxidation of atmospheric CH4. However, the Cl sink is highly fractionating, and thus strongly influences δ13C(CH4). As inversion studies do not prescribe the same Cl fields to constrain CH4 budget, it can lead to discrepancies between estimates. To quantify the influence of the Cl concentrations on CH4, δ13C(CH4) and CH4 budget estimates, we perform multiple sensitivity simulations using three Cl fields with concentrations that are realistic with regard to recent literature and one Cl field with concentrations that are very likely to be overestimated. We also test removing the tropospheric and the entire Cl sink in other sensitivity simulations. We find that the realistic Cl fields tested here are responsible for between 0.3 % and 1.8 % of the total chemical CH4 sink in the troposphere and between 1.0 % and 1.2 % in the stratosphere. Prescribing these different Cl amounts in surface-based inversions can lead to differences in global CH4 source adjustments of up to 12.3 TgCH4.yr−1. We also find that the globally-averaged isotopic signature of the CH4 sources inferred by a surface-based inversion assimilating δ13C(CH4) observations would decrease by 0.53 ‰ for each additional percent of contribution from the tropospheric Cl sink to the total sink. Finally, our study shows that CH4 seasonal cycle amplitude is modified by less than 1–2 % but δ13(CH4) seasonal cycle amplitude can be modified by up to 10–20 %, depending on the latitude.

scholarly journals Ambiguity in the causes for decadal trends in atmospheric methane and hydroxyl

2017 ◽  
Vol 114 (21) ◽  
pp. 5367-5372 ◽  
Author(s):  
Alexander J. Turner ◽  
Christian Frankenberg ◽  
Paul O. Wennberg ◽  
Daniel J. Jacob
Keyword(s):  
Greenhouse Gas ◽  
Recent Literature ◽  
Atmospheric Methane ◽  
Model Inversion ◽  
Sources And Sinks ◽  
Methyl Chloroform ◽  
Competing Hypotheses ◽  
Time Invariant ◽  
Global Mean ◽  
Methane Concentrations

Methane is the second strongest anthropogenic greenhouse gas and its atmospheric burden has more than doubled since 1850. Methane concentrations stabilized in the early 2000s and began increasing again in 2007. Neither the stabilization nor the recent growth are well understood, as evidenced by multiple competing hypotheses in recent literature. Here we use a multispecies two-box model inversion to jointly constrain 36 y of methane sources and sinks, using ground-based measurements of methane, methyl chloroform, and the C13/C12 ratio in atmospheric methane (δ13CH4) from 1983 through 2015. We find that the problem, as currently formulated, is underdetermined and solutions obtained in previous work are strongly dependent on prior assumptions. Based on our analysis, the mathematically most likely explanation for the renewed growth in atmospheric methane, counterintuitively, involves a 25-Tg/y decrease in methane emissions from 2003 to 2016 that is offset by a 7% decrease in global mean hydroxyl (OH) concentrations, the primary sink for atmospheric methane, over the same period. However, we are still able to fit the observations if we assume that OH concentrations are time invariant (as much of the previous work has assumed) and we then find solutions that are largely consistent with other proposed hypotheses for the renewed growth of atmospheric methane since 2007. We conclude that the current surface observing system does not allow unambiguous attribution of the decadal trends in methane without robust constraints on OH variability, which currently rely purely on methyl chloroform data and its uncertain emissions estimates.

scholarly journals Role of CO<sub>2</sub>, climate and land use in regulating the seasonal amplitude increase of carbon fluxes in terrestrial ecosystems: a multimodel analysis

2016 ◽  
Author(s):  
Fang Zhao ◽  
Ning Zeng ◽  
Ito Akihiko ◽  
Ghassam Asrar ◽  
Pierre Friedlingstein ◽  
...  
Keyword(s):  
Climate Change ◽  
Land Use ◽  
Seasonal Cycle ◽  
Decadal Variability ◽  
Model Ensemble ◽  
Co2 Fertilization ◽  
Dynamic Global Vegetation Model ◽  
Cross Model ◽  
Amplitude Increase ◽  
Atmospheric Inversions

Abstract. We examined the net terrestrial carbon flux to the atmosphere (FTA) simulated by nine models from the TRENDY dynamic global vegetation model project during 1961–2012 for its seasonal cycle and amplitude trend. While some models exhibit similar phase and amplitude compared to atmospheric inversions, with spring drawdown and autumn rebound, others tend to rebound early in summer. The model ensemble mean underestimates the magnitude of the seasonal cycle by 40 % compared to atmospheric inversions. Global FTA amplitude increase (19 ± 8 %) and its decadal variability from the model ensemble are generally consistent with constraints from surface atmosphere observations. However, models disagree on attribution of this long-term amplitude increase, with factorial experiments attributing 83 ± 56 %, −3 ± 74 % and 20 ± 30 % to rising CO2, climate change and land use/cover change, respectively. Seven out of the nine models suggest that CO2 fertilization is a stronger control — with the notable exception of VEGAS, which attributes approximately equally to the three factors. Generally, all models display an enhanced seasonality over the boreal region in response to high-latitude warming, but a negative climate contribution from part of the Northern Hemisphere temperate region, and the net result is a divergence over climate change effect. Six of the nine models show land use/cover change amplifies the seasonal cycle of global FTA: some are due to forest regrowth while others are caused by crop expansion or agricultural intensification, as revealed by their divergent spatial patterns. We also discovered a moderate cross-model correlation between FTA amplitude increase and increase in land carbon sink (R2 = 0.61). Our results suggest that models can show similar results in some benchmarks with different underlying mechanisms, therefore the spatial traits of CO2 fertilization, climate change, and land use/cover changes are crucial in determining the right mechanisms in seasonal carbon cycle change as well as mean sink change.

scholarly journals Variability and quasi-decadal changes in the methane budget over the period 2000–2012

2017 ◽  
Author(s):  
Marielle Saunois ◽  
Philippe Bousquet ◽  
Benjamin Poulter ◽  
Anna Peregon ◽  
Philippe Ciais ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Methane Emissions ◽  
Data Driven ◽  
Atmospheric Methane ◽  
Top Down ◽  
Bottom Up ◽  
Ch4 Emissions ◽  
Ensemble Mean ◽  
The Mean ◽  
The Tropics

Abstract. Following the recent Global Carbon project (GCP) synthesis of the decadal methane (CH4) budget over 2000–2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling frameworks) and bottom-up models, inventories, and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000–2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000–2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008–2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16–32] Tg CH4 yr−1 higher methane emissions over the period 2008–2012 compared to 2002–2006. This emission increase mostly originated from the tropics with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seems to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002–2006 and 2008–2012 differs from one atmospheric inversion study to another. However, all top-down studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the EDGARv4.2 inventory, which should be revised to smaller values in a near future. Though the sectorial partitioning of six individual top-down studies out of eight are not consistent with the observed change in atmospheric 13CH4, the partitioning derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that, the dominant contribution to the resumed atmospheric CH4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH4 emissions. Besides, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric 13CH4 observations. The methane loss (in particular through OH oxidation) has not been investigated in detail in this study, although it may play a significant role in the recent atmospheric methane changes.

scholarly journals Changes Of Atmospheric Methane Concentration Parallel To Climatic Changes

1990 ◽  
Vol 14 ◽  
pp. 359-359
Author(s):  
B. Stauffer ◽  
H. Oeschger ◽  
J. Schwander
Keyword(s):  
Climatic Change ◽  
Methane Concentration ◽  
Ice Core ◽  
Younger Dryas ◽  
Climatic Changes ◽  
Atmospheric Methane ◽  
Sources And Sinks ◽  
Core Samples ◽  
Climatic Optimum ◽  
Present Understanding

Measurements on ice-core samples showed that atmospheric methane concentration changed with the large climatic cycles during the last two glaciations (Stauffer and others, 1988; Raynaud and others, 1988). The methane concentration is lower in cold periods and higher in warm periods. In this paper we discuss the results of CH4 measurements of samples from periods of minor climatic change, like the climatic optimum 8000 years B.P. and the Younger Dryas period about 10 000 to 11 000 years B.P.. The data are interpreted in terms of the present understanding of methane sources and sinks.

scholarly journals Changes Of Atmospheric Methane Concentration Parallel To Climatic Changes

1990 ◽  
Vol 14 ◽  
pp. 359
Author(s):  
B. Stauffer ◽  
H. Oeschger ◽  
J. Schwander
Keyword(s):  
Climatic Change ◽  
Methane Concentration ◽  
Ice Core ◽  
Younger Dryas ◽  
Climatic Changes ◽  
Atmospheric Methane ◽  
Sources And Sinks ◽  
Core Samples ◽  
Climatic Optimum ◽  
Present Understanding

Measurements on ice-core samples showed that atmospheric methane concentration changed with the large climatic cycles during the last two glaciations (Stauffer and others, 1988; Raynaud and others, 1988). The methane concentration is lower in cold periods and higher in warm periods. In this paper we discuss the results of CH4 measurements of samples from periods of minor climatic change, like the climatic optimum 8000 years B.P. and the Younger Dryas period about 10 000 to 11 000 years B.P.. The data are interpreted in terms of the present understanding of methane sources and sinks.

scholarly journals Description and Evaluation of the specified-dynamics experiment in the Chemistry-Climate Model Initiative

2020 ◽  
Vol 20 (6) ◽  
pp. 3809-3840 ◽  
Author(s):  
Clara Orbe ◽  
David A. Plummer ◽  
Darryn W. Waugh ◽  
Huang Yang ◽  
Patrick Jöckel ◽  
...  
Keyword(s):  
Seasonal Cycle ◽  
General Circulation ◽  
Large Scale ◽  
Climate Model ◽  
Phase 1 ◽  
General Circulation Models ◽  
Atmospheric Composition ◽  
Cycle Amplitude ◽  
Free Running ◽  
Dynamics Simulations

Abstract. We provide an overview of the REF-C1SD specified-dynamics experiment that was conducted as part of phase 1 of the Chemistry-Climate Model Initiative (CCMI). The REF-C1SD experiment, which consisted of mainly nudged general circulation models (GCMs) constrained with (re)analysis fields, was designed to examine the influence of the large-scale circulation on past trends in atmospheric composition. The REF-C1SD simulations were produced across various model frameworks and are evaluated in terms of how well they represent different measures of the dynamical and transport circulations. In the troposphere there are large (∼40 %) differences in the climatological mean distributions, seasonal cycle amplitude, and trends of the meridional and vertical winds. In the stratosphere there are similarly large (∼50 %) differences in the magnitude, trends and seasonal cycle amplitude of the transformed Eulerian mean circulation and among various chemical and idealized tracers. At the same time, interannual variations in nearly all quantities are very well represented, compared to the underlying reanalyses. We show that the differences in magnitude, trends and seasonal cycle are not related to the use of different reanalysis products; rather, we show they are associated with how the simulations were implemented, by which we refer both to how the large-scale flow was prescribed and to biases in the underlying free-running models. In most cases these differences are shown to be as large or even larger than the differences exhibited by free-running simulations produced using the exact same models, which are also shown to be more dynamically consistent. Overall, our results suggest that care must be taken when using specified-dynamics simulations to examine the influence of large-scale dynamics on composition.

scholarly journals Strong Sensitivity of the Isotopic Composition of Methane to the Plausible Range of Tropospheric Chlorine

2019 ◽  
Author(s):  
Sarah A. Strode ◽  
James S. Wang ◽  
Michael Manyin ◽  
Bryan Duncan ◽  
Ryan Hossaini ◽  
...  
Keyword(s):  
Geographic Distribution ◽  
Seasonal Cycle ◽  
Isotopic Ratio ◽  
Chemical Transport ◽  
Transport Models ◽  
Chemical Transport Models ◽  
Highly Sensitive ◽  
Fixed Set ◽  
Additional Constraints ◽  
Methane Sink

Abstract. The 13C isotopic ratio of methane, δ13C of CH4, provides additional constraints on the CH4 budget to complement the constraints from CH4 observations. The interpretation of δ13C observations is complicated, however, by uncertainties in the methane sink. The reaction of CH4 with Cl is highly fractionating, increasing the relative abundance of 13CH4, but there is currently no consensus on the strength of the tropospheric Cl sink. We use a set of GEOS global model simulations with different predicted Cl fields to test the sensitivity of the δ13C of CH4 to the diversity of Cl output from chemical transport models. We find that δ13C is highly sensitive to both the amount and geographic distribution of Cl. Simulatlons with Cl providing 0.28 % or 0.66 % of the total CH4 loss bracket the δ13C observations for a fixed set of emissions. Thus, even when Cl provides only a small fraction of the total CH4 loss and has a small impact on total CH4, it provides a strong lever on δ13C. The geographic distribution and seasonal cycle of Cl also impacts the hemispheric gradient and seasonal cycle of δ13C. The large effect of Cl on δ13C compared to total CH4 broadens the range of CH4 source mixtures that can be reconciled with δ13C observations. Stronger constraints on tropospheric Cl are necessary to improve estimates of CH4 sources from δ13C observations.

scholarly journals On the Physical Origin of the Semiannual 1 Component of Surface Air Temperature over 2 Mid-latitude and Subpolar Oceans

2021 ◽  
Author(s):  
Fucheng Yang ◽  
Zhaohua Wu
Keyword(s):  
Heat Capacity ◽  
Air Temperature ◽  
Mixed Layer ◽  
Solar Irradiance ◽  
Seasonal Cycle ◽  
Surface Air Temperature ◽  
Physical Origin ◽  
Oceanic Mixed Layer ◽  
Sources And Sinks ◽  
Yearly Period

Abstract With the understanding that seasonal cycle of the temperature are forced principally by the annually evolving solar irradiance, many previous studies have defined seasonal cycle of surface air temperature (SAT) as the sum of yearly-period sinusoidal component and its harmonics, especially semiannual component. In mid-latitude and subpolar regions, the ratio between the semiannual and annual components of solar irradiance is negligibly small but that of the SAT over oceans is not, which remains to be understood. In this study, a simple energy budget model including main energy sources and sinks of oceanic mixed layer is designed to understand this puzzle. It is revealed that, when the oceanic mixed layer is prescribed as a layer of constant depth, the phase and amplitude of the modeled SAT is not consistent with that of the observation. However, when the annually changing heat capacity of the oceanic mixed layer is included, both the amplitude and phase of the modeled SAT share these of the observed SAT, proving that the semiannual component of SAT over mid-latitude and subpolar oceans is a result of the heat capacity-varying oceanic mixed layer in response to annually evolving solar irradiance.

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